Optimal control in a dissipative system: Vibrational excitation of CO∕Cu(100) by IR pulses

摘要: The question as to whether state-selective population of molecular vibrational levels by shaped infrared laser pulses is possible in a condensed phase environment central importance for such diverse fields time-resolved spectroscopy, quantum computing, or “vibrationally mediated chemistry.” This addressed here model system, representing carbon monoxide adsorbed on Cu(100) surface. Three the six modes are considered explicitly, namely, CO stretch vibration, CO-surface and frustrated translation. Optimized excitation “bright” “dark” designed optimal control theory framework Markovian open-system density matrix approach, with energy flow substrate electrons phonons, relaxation, finite temperature accounted for. analyzed their Husimi “quasiprobability” distribution time-energy space.